Recent exploitations of the superior mechanical and electronic properties of carbon nanotubes (CNTs) have led to exciting opportunities in low-cost, high performance, carbon-based electronics. In this report, low-voltage thin-film transistors with aligned, semiconducting CNT networks are fabricated on a chemically modified polymer gate dielectric using both rigid and flexible substrates. The multifunctional polymer serves as a thin, flexible gate dielectric film, affords low operating voltages, and provides a platform for chemical functionalization. The introduction of amine functionality to the dielectric surface leads to the adsorption of a network enriched with semiconducting CNTs with tunable density from spin coating a bulk solution of unsorted CNTs. The composition of the deposited CNT networks is verified with Raman spectroscopy and electrical characterization. For transistors at operating biases below 1 V, we observe an effective device mobility as high as 13.4 cm(2)/Vs, a subthreshold swing as low as 130 mV/dec, and typical on-off ratios of greater than 1,000. This demonstration of high performance CNT thin-film transistors operating at voltages below 1 V and deposited using solution methods on polymeric and flexible substrates is an important step toward the realization of low-cost flexible electronics.